Chinese Journal of Catalysis ›› 2018, Vol. 39 ›› Issue (7): 1249-1257.DOI: 10.1016/S1872-2067(18)63058-X

• Article • Previous Articles     Next Articles

Superior performance of Co-N/m-C for direct oxidation of alcohols to esters under air

Ning Lia,b, Sensen Shangb, Lianyue Wangb, Jingyang Niua, Ying Lvb, Shuang Gaob   

  1. a Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, Henan, China;
    b Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • Received:2018-01-09 Revised:2018-02-24 Online:2018-07-18 Published:2018-06-07
  • Contact: 10.1016/S1872-2067(18)63058-X
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21773232, 21403219, 21773227).

Abstract:

A convenient, expeditious, and high-efficiency protocol for the transformation of alcohols into esters using a Co-modified N-doped mesoporous carbon material (Co-N/m-C) as the catalyst is proposed. The catalyst was prepared through direct pyrolysis of a macromolecular precursor. The catalyst prepared using a pyrolysis temperature of 900℃ (labeled Co-N/m-C-900) exhibited the best performance. The strong coordination between the ultra-dispersed cobalt species and the pyridine nitrogen as well as the large area of the mesoporous surface resulted in a high turnover frequency value (107.6 mol methyl benzoate mol-1 Co h-1) for the direct aerobic oxidation of benzyl alcohol to methyl benzoate. This value is much higher than those of state-of-the-art transition-metal-based nanocatalysts reported in the literature. Moreover, the catalyst exhibited general applicability to various structurally diverse alcohols, including benzylic, allylic, and heterocyclic alcohols, achieving the target esters in high yields. In addition, a preliminary evaluation revealed that Co-N/m-C-900 can be used six times without significant activity loss. In general, the process was rapid, simple, and cost-effective.

Key words: Cobalt, N-doped, Mesoporous carbon, Esters, Catalysis